Formation of charge-polarized regions at dual single-atom sites for C-H bond activation in methane.

Direct conversion of CH into liquid oxygenates under mild conditions is of great significance but remains challenging due to the high dissociation energy of inert C-H bond. Here we report the fabrication of a dual atomic Fe and Pd catalyst with periodic macroporous structure (Fe-Pd OMNC) toward the direct CH conversion at room temperature. Mechanism studies reveal that a charge polarization region (O-Fe-Pd) is formed in-situ on Fe-Pd atomic sites upon oxidant activation, wherein the electron-rich O and electron-deficient Pd regions can respectively capture the H and CH in CH and lead to the activation of C-H bond. As a result, Fe-Pd OMNC demonstrates attractive photothermal catalytic performance toward the selective oxidation of CH under Xe lamp irradiation, achieving the productivities of C1 oxygenates as high as 0.754 mmol h and 0.035 mmol h when using HO or O as the oxidant, respectively.